A catalytic technique to enhance graphite formation in nongraphitizing carbons was adapted to work with three-dimensional wood-derived scaffolds. Unlike many synthetic graphite precursors, wood and other cellulosic carbons remain largely disordered after high temperature pyrolysis. Using a nickel nitrate liquid catalyst and controlled pyrolysis conditions, wood-derived scaffolds were produced showing similar graphitic content to traditional pitch-based graphite while retaining the high-aspect ratio pores of the precursor wood microstructure. Graphite formation was studied as a function of processing time and pyrolysis temperature, and the resulting carbons were analyzed using x-ray diffraction, Raman spectroscopy, x-ray photoelectron spectroscopy, and electron microscopy techniques.